Matsumoto Hikaru, Seto Hirokazu, Akiyoshi Takanori, Shibuya Makoto, Hoshino Yu, Miura Yoshiko
Department of Chemical Engineering, Kyushu University, 744 Motooka, Nishi-ku, Fukuoka 819-0395, Japan.
Department of Chemical Engineering, Fukuoka University, 8-19-1 Nanakuma, Jonan-ku, Fukuoka 814-0180, Japan.
ACS Omega. 2017 Dec 8;2(12):8796-8802. doi: 10.1021/acsomega.7b00909. eCollection 2017 Dec 31.
We mimic a living system wherein target molecules permeate through capillary and cells for chemical transformation. A monolithic porous gel (MPG) was easily prepared by copolymerization of gel matrix, tertiary amine, and cross-linking monomer in one-step synthesis. Interconnected capillaries existed in the MPG, enabling flow application with high permeability. Because the capillaries were constituted of polymer gel, Pd(0)-loaded MPG provided another permeable pathway to substrates in a gel network, contributing to its much high turnover number after 30 days of use, compared with that of Pd(0)-loaded inorganic supports. Interestingly, the gel network size of the MPG influenced the catalytic frequency. Diffusivities of the substrates and product in the gel networks increased with increasing network sizes in relation to catalytic activities. The MPG strategy provides a universal reactor design in conjunction with a practical process and precisely controlled reaction platform.
我们模拟了一个生物系统,其中目标分子通过毛细血管和细胞进行化学转化。通过在一步合成中使凝胶基质、叔胺和交联单体共聚,轻松制备了整体式多孔凝胶(MPG)。MPG中存在相互连接的毛细血管,使其具有高渗透性,能够进行流动应用。由于毛细血管由聚合物凝胶构成,负载Pd(0)的MPG在凝胶网络中为底物提供了另一条渗透途径,与负载Pd(0)的无机载体相比,使用30天后其周转数要高得多。有趣的是,MPG的凝胶网络尺寸影响催化频率。底物和产物在凝胶网络中的扩散系数随着网络尺寸的增加而增加,与催化活性相关。MPG策略结合实际工艺和精确控制的反应平台,提供了一种通用的反应器设计。